The bulk of the Smith collection - the Chronological Series - has been arranged first by years, and then alphabetically within the year, so that except for the earlier years when groups of materials have been brought together, an alphabetical series exists for each year from 1943 to 1976. The amount of material for each year varies depending upon Smith's activities, but usually averages 3 to 4 linear feet. Inexplicably, the files for 1966 and 1967 are fragmentary, and may have been destroyed or mislaid. This series includes all types of materials, but consists primarily of correspondence. The file headings used are the names of individuals with whom Smith corresponded, organizations and issues in which he was interested, and places where Smith and his organization held meetings. There is also a miscellaneous folder for each letter of the alphabet.

The subjects covered in the Chronological Series reflect Smith's own interests and activities. In general terms, the files concern the relationship between Smith and his ideological supporters, between Smith and his staff, attorneys, and those responsible for meeting arrangements and for the publication and distribution of the Cross and the Flag and other newsletters. Of special note are exchanges of letters between Smith and the many individuals who held contrary views.

The Chronological Series is particularly valuable for information that it provides about the informal network and linkages among conservative organizations and individuals. Smith corresponded widely, and he and his staff collected material on the work of other conservatives, abroad as well as in the United States. Some of these individuals became closely associated with Smith and his work, speaking at his rallies or writing for the Cross and the Flag. Others started out with the Smith organization, then split off for ideological reasons or personal differences with Smith. Because Smith was a national figure, his files document conservative and anti-Zionist causes in many regions of the country and over a fairly broad period of time, 1940-1976. Correspondents and organizations represented in the collection include: George W. Armstrong (head of the Judge Armstrong Foundation for the furtherance of a unified anti-Semitic movement), John O. Beaty (university teacher and author of The Iron Curtain over America), Mrs. Catherine Brown (head of the National Blue Star Mothers of America), Elizabeth Dilling (anti-Communist crusader and director of the Patriotic Research Bureau), Myron C. Fagan (national director of the anti-Communist, Cinema Educational Guild), Kenneth Goff (pastor and head of various anti-Communist organizations in Colorado), Norman Jaques (Canadian M.P. and supporter of Smith and his work), Frederick Kister (director of the Christian Veterans of America), Conde McGinley (editor of anti-Communist newspaper, Common Sense), Leland Marion (pastor, and candidate for governor of Michigan in 1944 on the America First ticket), Jonathan E. Perkins (Los Angeles pastor and supporter of Smith), Harvey H. Springer (Colorado pastor and editor of Western Voice), Jack B. Tenney (California state senator and candidate for vice-president on the Christian National Party ticket in 1952), Rev. A. W. Terminiello ("Father Coughlin of the South," secretary of the Union of Christian Crusaders), Gerald P. Winrod (prominent pastor and publisher of Christian, anti Communist journal, The Defender).

In addition, the Smith correspondence files contain letters from significant individuals who had no direct ties to Smith buy were responding to queries from Smith, or who were seeking Smith's advice. Smith sometimes initiated correspondence with individuals, either to castigate or compliment them, or just to spread his own views more broadly. Such correspondence is usually not extensive, but the letters are always of interest. Such correspondents include: H.L. Mencken, William F. Buckley, Gamal Abdul Nasser, Robert Welch, George Lincoln Rockwell, Westbrook Pegler, George Sokolsky, Arthur Vandenberg, and Ernest Liebold (secretary to Henry Ford).